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弥合分子质谱与元素质谱之间的差距:高能碰撞解离(HCD)揭示元素信息。

Bridging the gap between molecular and elemental mass spectrometry: higher energy collisional dissociation (HCD) revealing elemental information.

作者信息

Esteban-Fernández Diego, El-Khatib Ahmed H, Moraleja Irene, Gómez-Gómez M Milagros, Linscheid Michael W

机构信息

Department of Chemistry, Humboldt-Universitaet zu Berlin , Brook-Taylor Str. 2, 12489, Berlin, Germany.

出版信息

Anal Chem. 2015 Feb 3;87(3):1613-21. doi: 10.1021/ac5032447. Epub 2015 Jan 15.

DOI:10.1021/ac5032447
PMID:25528895
Abstract

Molecular mass spectrometry has been applied to simultaneously obtain molecular and elemental information from metal-containing species. Energy tuning of the higher-energy collision dissociation (HCD) fragmentation cell allows the controlled production of typical peptide fragments or elemental reporter ions informing about the metallic content of the analyzed species. Different instrumental configurations and fragmentation techniques have been tested, and the efficiency extracting the elemental information has been compared. HCD fragmentation operating at very high energy led to the best results. Platinum, lanthanides, and iodine reporter ions from peptides interacting with cisplatin, peptides labeled with lanthanides-MeCAT-IA, and iodinated peptides, respectively, were obtained. The possibility to produce abundant molecular and elemental ions in the same analysis simplifies the correlation between both signals and open pathways in metallomics studies enabling the specific tracking of metal-containing species. The proposed approach has been successfully applied to in solution standards and complex samples. Moreover, interesting preliminary MALDI-imaging experiments have been performed showing similar metal distribution compared to laser ablation (LA)-ICPMS.

摘要

分子质谱已被用于同时从含金属物种中获取分子和元素信息。高能碰撞解离(HCD)碎裂池的能量调谐允许可控地产生典型的肽片段或元素报告离子,从而获知被分析物种的金属含量。已经测试了不同的仪器配置和碎裂技术,并比较了提取元素信息的效率。在非常高的能量下运行的HCD碎裂产生了最佳结果。分别从与顺铂相互作用的肽、用镧系元素-MeCAT-IA标记的肽和碘化肽中获得了铂、镧系元素和碘报告离子。在同一分析中产生大量分子和元素离子的可能性简化了两种信号之间的相关性,并为金属组学研究开辟了途径,能够对含金属物种进行特异性追踪。所提出的方法已成功应用于溶液标准品和复杂样品。此外,已经进行了有趣的基质辅助激光解吸电离成像(MALDI-成像)实验,结果显示与激光烧蚀电感耦合等离子体质谱(LA-ICPMS)相比,金属分布相似。

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